Despite the key role that ionic solutions play in several natural and industrial processes, a unified, molecular-level understanding of how ions affect the structure and dynamics of water across different phases remains elusive. In this context, computer simulations can provide new insights that are difficult, if not impossible, to obtain by other means. However, the predictive power of a computer simulation directly depends on the level of ‘realism’ that is used to represent the underlying molecular interactions. Here, we report a systematic analysis of many-body effects in halide-water clusters and demonstrate that the recently developed MB-nrg full-dimensional many-body potential energy functions achieve high accuracy by quantitatively reproducing the individual terms of the many-body expansion of the interaction energy, thus opening the door to realistic computer simulations of ionic solutions.

尽管离子溶液在几种自然和工业过程中起着关键作用，但是对于离子如何影响不同相中水的结构和动力学的统一，分子水平的了解仍然难以捉摸。在这种情况下，计算机模拟可以提供新的见解，而这些见解即使不是不可能的，也很难通过其他方式获得。但是，计算机模拟的预测能力直接取决于用于表示基本分子相互作用的“现实”水平。在这里，我们报告了卤化物-水团簇中多体效应的系统分析，并证明了最近开发的MB-nrg全维多体势能函数通过定量再现多体膨胀的各个项而实现了高精度。的相互作用能